The tie-up will see Barclays take over as the competition's backer from next season at a cost of £19m a year. Running until the end of the 2006-07 season, it will allow the group to associate the Premier League with its entire business portfolio.
Barclays was the sponsor of the Football League from 1987 until 1993.
The Premier League was formed in 1992 and was not covered by the Barclays deal.
The agreement, which was rubber-stamped at a meeting of the Premiership's 20 clubs, will see Barclays installed as the sponsor of the Premier League's proposed community coaching programme, cementing its grass-roots sponsorship.
Barclaycard chief executive Gary Hoffman and his Premier League counterpart, Richard Scudamore, hailed the sponsorship as an exciting development and an indication of the Barclays group's commitment to football.
"It fits our international presence and provides us with powerful brand visibility around the world, as well as the type of platform we need to further establish the Barclays name at home and abroad," said Hoffman.
Bucking the trend of a sponsorship market that has seen the value of many sporting properties plunge during the economic downturn, the Premier League sponsorship remains highly sought-after because of English football's worldwide popularity. The current three-year deal, signed after Carling ended its nine-year association in 2001, is worth about £16m a year.
The launch of the sponsorship will coincide with the advent of the Premier League's £1bn TV rights deal, which is under scrutiny from the European Commission after BSkyB won the right to show an unprecedented number of live matches.
The Premier League has also announced that Vodafone and 3 have been jointly awarded mobile rights for the next three seasons.
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